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  • Muller, David A  (2)
  • Padgett, Elliot  (2)
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  • 1
    Online Resource
    Online Resource
    Oxford University Press (OUP) ; 2023
    In:  Microscopy and Microanalysis Vol. 29, No. 4 ( 2023-07-25), p. 1422-1435
    In: Microscopy and Microanalysis, Oxford University Press (OUP), Vol. 29, No. 4 ( 2023-07-25), p. 1422-1435
    Abstract: Measuring local polar ordering is key to understanding ferroelectricity in thin films, especially for systems with small domains or significant disorder. Scanning nanobeam electron diffraction (NBED) provides an effective local probe of lattice parameters, local fields, polarization directions, and charge densities, which can be analyzed using a relatively low beam dose over large fields of view. However, quantitatively extracting the magnitudes and directions of polarization vectors from NBED remains challenging. Here, we use a cepstral approach, similar to a pair distribution function, to determine local polar displacements that drive ferroelectricity from NBED patterns. Because polar distortions generate asymmetry in the diffraction pattern intensity, we can efficiently recover the underlying displacements from the imaginary part of the cepstrum transform. We investigate the limits of this technique using analytical and simulated data and give experimental examples, achieving the order of 1.1 pm precision and mapping of polar displacements with nanometer resolution.
    Type of Medium: Online Resource
    ISSN: 1431-9276 , 1435-8115
    Language: English
    Publisher: Oxford University Press (OUP)
    Publication Date: 2023
    detail.hit.zdb_id: 1481716-0
    SSG: 11
    SSG: 12
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  • 2
    Online Resource
    Online Resource
    The Electrochemical Society ; 2023
    In:  ECS Meeting Abstracts Vol. MA2023-01, No. 38 ( 2023-08-28), p. 2259-2259
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2023-01, No. 38 ( 2023-08-28), p. 2259-2259
    Abstract: Interest is growing in applying fuel cells to heavy duty transportation applications, which requires the fuel cell design to prioritize efficiency and durability to provide a low lifetime cost of ownership. This motivates further development of catalysts for the oxygen reduction reaction (ORR), as ORR kinetics are a key factor in fuel cell efficiency and catalyst degradation is a major factor limiting lifetime. Pt-alloy catalysts have seen success in light-duty fuel cell applications, where they provide enhanced activity believed to originate (at least in part) from strain of the active Pt surface by the underlying Pt-alloy core. Concerns remain regarding the viability of PtCo catalysts for heavy duty applications, as they may not sustain their activity advantage over extended lifetimes and leaching of the base metal can lead to additional performance degradation. These concerns motivate investigation into the fundamental mechanisms of strain-induced activity enhancements to guide further catalyst development and understand the ultimate limits for the performance and stability of PtCo catalysts. However, practical Pt-alloy fuel cell catalysts are complex, and understanding of real strain effects in these systems remains elusive. Here we will present an investigation into strain effects in Pt-Co ORR catalysts for fuel cells, combining scanning nanobeam electron diffraction (NBED), continuum elastic strain modelling, and full-cell electrochemistry measurements. We leverage recent developments in NBED to make high-throughput strain maps in heterogeneous, carbon-supported PtCo catalysts and identify different mechanisms of strain relaxation, including dislocations and geometric effects. Supported by continuum elastic modelling, we correlate shell thickness, strain state, and activity of PtCo catalysts. Finally, we will comment on how these results provide rational guidance to optimize stable, efficient Pt-alloy catalysts.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2023
    detail.hit.zdb_id: 2438749-6
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